Abstract
Polarized single crystal absorption spectra are reported for three nickel complexes: bis‐N‐methylsalicylaldiminato‐nickel (II), bis‐salicylaldiminato‐nickel (II), and diaquo‐bis‐salicylaldehydato‐nickel (II). The analysis of the bands of an orthorhombic form of bis‐N‐methyl‐salicylaldiminato‐nickel (II) (described for the first time) results in the assignment of the two visible absorption bands to 1Ag1B1g and 1Ag1B3g, respectively. This assignment is discussed in relation to the simple crystal field model and a possible refinement of the model has been suggested. The analysis of the band observed with bis‐salicylaldiminato‐nickel (II) is consistent with the assignment of those in bis‐N‐methylsalicylaldiminato‐nickel (II). The analysis of the visible absorption band of diaquo‐bis‐salicylaldehydato‐nickel (II) shows that the theoretical assignment is incorrect although an unambiguous assignment cannot be made from the crystal spectrum.

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